We apply the self-healing diffusion Monte Carlo algorithm
(SHDMC) [Phys. Rev. B {\bf 79} 195117 (2009), ibid. {\bf 80}
125110 (2009)] to
the calculation of ground states of atoms and
molecules. By comparing with configuration
interaction results we show the method yields systematic
convergence towards the exact ground state wave function and
reduction of the fixed-node DMC sign error. We present results
for atoms and light molecules, obtaining, e.g. the
binding of N$_2$ to chemical accuracy. Moreover, we
demonstrate that the algorithm is robust enough to be used for
the systems as large as the fullerene
C$_{20}$ starting from a set of random coefficients. SHDMC thus
constitutes a practical method for systematically reducing the
Fermion sign problem in electronic structure calculations.
Research sponsored by the ORNL LDRD program (MB), U.S. DOE BES
Divisions of Materials Sciences \& Engineering (FAR, MLT) and
Scientific User Facilities (PRCK). LLNL research was performed
under U.S. DOE contract DE-AC52-07NA27344 (RQH).

To cite this abstract, use the following reference: http://meetings.aps.org/link/BAPS.2010.MAR.H23.9